| Summary: | The rapidly growing Li-ion battery market has generated considerable demand for Li-ion batteries with improved performance and stability. All-solid-state Li-ion batteries offer promising safety and manufacturing enhancements. Herein, we examine the effect of substitutional doping at three cation sites in garnet-type Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO) oxide ceramics produced by a sol–gel synthesis technique with the aim of enhancing the properties of solid-state electrolytes for use in all-solid-state Li-ion batteries. Building on the results of mono-doping experiments with different doping elements and sites—Al, Ga, and Ge at the Li<sup>+</sup> site; Rb at the La<sup>3+</sup> site; and Ta and Nb at the Zr<sup>4+</sup> site—we designed co-doped (Ga, Al, or Rb with Nb) and tri-doped (Ga or Al with Rb and Nb) samples by compositional optimization, and achieved a LLZO ceramic with a pure cubic phase, almost no secondary phase, uniform grain structure, and excellent Li-ion conductivity. The findings extend the current literature on the doping of LLZO ceramics and highlight the potential of the sol–gel method for the production of solid-state electrolytes.
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